US8475729B2 - Methods for forming honeycomb minireactors and systems - Google Patents

Methods for forming honeycomb minireactors and systems Download PDF

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US8475729B2
US8475729B2 US12/623,737 US62373709A US8475729B2 US 8475729 B2 US8475729 B2 US 8475729B2 US 62373709 A US62373709 A US 62373709A US 8475729 B2 US8475729 B2 US 8475729B2
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cells
path
reactor
pattern
cell
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US20100132928A1 (en
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James Scott Sutherland
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Corning Inc
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Corning Inc
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B21—MECHANICAL METAL-WORKING WITHOUT ESSENTIALLY REMOVING MATERIAL; PUNCHING METAL
    • B21D—WORKING OR PROCESSING OF SHEET METAL OR METAL TUBES, RODS OR PROFILES WITHOUT ESSENTIALLY REMOVING MATERIAL; PUNCHING METAL
    • B21D53/00—Making other particular articles
    • B21D53/02—Making other particular articles heat exchangers or parts thereof, e.g. radiators, condensers fins, headers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/248—Reactors comprising multiple separated flow channels
    • B01J19/2485—Monolithic reactors
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F28—HEAT EXCHANGE IN GENERAL
    • F28F—DETAILS OF HEAT-EXCHANGE AND HEAT-TRANSFER APPARATUS, OF GENERAL APPLICATION
    • F28F21/00—Constructions of heat-exchange apparatus characterised by the selection of particular materials
    • F28F21/04—Constructions of heat-exchange apparatus characterised by the selection of particular materials of ceramic; of concrete; of natural stone
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F28—HEAT EXCHANGE IN GENERAL
    • F28F—DETAILS OF HEAT-EXCHANGE AND HEAT-TRANSFER APPARATUS, OF GENERAL APPLICATION
    • F28F7/00—Elements not covered by group F28F1/00, F28F3/00 or F28F5/00
    • F28F7/02—Blocks traversed by passages for heat-exchange media
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T29/00—Metal working
    • Y10T29/49—Method of mechanical manufacture
    • Y10T29/49345—Catalytic device making
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T29/00—Metal working
    • Y10T29/49—Method of mechanical manufacture
    • Y10T29/4935—Heat exchanger or boiler making

Definitions

  • the present invention relates generally to honeycomb or extruded-body based reactors, more specifically to systems and methods for maximizing the utility and minimizing the cost of honeycomb reactors for a wide range of heat exchange and other performance requirements.
  • a method of forming a honeycomb reactor or reactor component including the steps of providing a honeycomb structure having cells divided by cell walls, providing and array of cutting tools arrayed in a pattern so as to be able to simultaneously align with a first plurality of the cell walls at a first end of the structure, and cutting the walls of the first plurality with the array of cutting tools, reducing the height of the cell walls of the first plurality.
  • Other aspects of the invention include reactors and/or systems formed of such reactors or reactor components and methods of use, including standardized reactor or reactor component systems, and standardized reactor or reactor component engineering or design.
  • FIG. 1 is a plan view of reactor or reactor component comprising a honeycomb body showing a path of a fluid passage, taken in a plane perpendicular to the common direction of the cells.
  • FIGS. 2 and 2A are side elevation views of the reactor or reactor component of FIG. 1 , showing path details in a plane parallel to the common direction of the cells, of the fluid passage of FIG. 1 according to two different embodiments thereof.
  • FIGS. 3 , 4 , and 4 A are is a cross-sectional views of cells closed on one or both ends of a honeycomb body, showing various methods useful in the context of the present invention for interconnection between cells.
  • FIG. 5 is a plan view of reactor or reactor component comprising a honeycomb body showing an alternative path of a fluid passage, taken in the plane perpendicular to the common direction of the cells, with end-face access to the fluid passage.
  • FIG. 6 is a perspective view of a reactor or reactor component having a fluid passage path, in the plane perpendicular to the cells, similar to the reactor of FIG. 5 , but with side access to the passage.
  • FIG. 7 is a cross-sectional view of a reactor or reactor component showing an instance of fluid connections to the end face of the extruded body.
  • FIG. 8 is a cross-sectional view of a reactor or reactor component showing fluid connections to side faces of the extruded body.
  • FIGS. 9 , 10 , 11 , 12 , 13 , 14 , 14 A, 15 , 16 , 17 , 18 , 19 , 20 , 21 , 22 , 23 , 24 , 25 , 26 , 27 , 28 , 29 , and 30 are semi-schematic plan view diagrams of path patterns, taken in a plane perpendicular to the common cell direction, including repeating path-units, useful in the context of the present invention.
  • FIG. 31 is a graph comparing certain performance parameters of the patterns of FIGS. 9-30 .
  • FIG. 32 is a graph comparing a certain performance metric of the patterns of FIGS. 9-30 .
  • FIG. 33 is a semi-schematic plan view of an array of cutting tools useful for manufacturing reactors or reactor components according to one aspect of the present invention.
  • FIG. 34 is a diagrammatic side elevation view of an apparatus for manufacturing reactors or reactor components according to another aspect of the present invention.
  • FIG. 35 is a diagrammatic side elevation view of another apparatus for manufacturing reactors or reactor components according to another aspect of the present invention.
  • FIG. 36 is a cross section of a portion of a reactor or reactor system according to yet another aspect of the present invention.
  • FIG. 1 shows a plan view of a type of reactor or reactor component 12 with which the present invention is concerned.
  • FIG. 2 shows a perspective view of the reactor or reactor component 12
  • FIG. 2A shows perspective view of an alternative embodiment.
  • the reactor or reactor component 12 comprises a honeycomb body 20 .
  • the body 20 has cells 23 extending in parallel in a common direction from a first end 32 of the body to a second end 34 , with the cells 23 seen end-on in FIG. 1 , divided by walls 82 .
  • the cells 23 include a first plurality of cells 22 open at both ends of the body and a second plurality of cells 24 closed at one or both ends of the body, such as, in this example, by one or more plugs 26 or by a more or less continuous plugging material 26 disposed at or near the end of the body and optionally partly within the cells of the second plurality of cells 24 .
  • the second plurality of cells 24 (the closed cells) contain a passage 28 extending through the body 20 across the cells 24 .
  • the passage 28 may follow a serpentine path 29 up and down along the common direction of the cells 23 , in the general direction shown in FIG. 2 , extending laterally perpendicular to the cells 23 only at or near the ends 32 , 34 of the body 20 , where walls between the cells 24 are shortened to allow fluid communication between the cells 24 .
  • the passage 28 or path 29 need not follow a serpentine path back and forth along the common direction, but follows instead a wide, parallel path across the cells 24 whose walls have been removed completely or in major part, as suggested by the path 29 of FIG. 2A .
  • Further variations may be used, such as passage paths having lower-frequency serpentines, for example. Example cross-sections of such embodiments are given in FIGS. 3 and 4 . If the passage 28 or path 29 is serpentine in the direction shown in FIG. 2 , the passage 28 or path 29 may follow a single cell up and down in the common direction along the cells 24 , as shown in FIG. 3 .
  • the passage 28 or path 29 may follow multiple successive respective groups of two or more cells in parallel, in the common direction along the cells 24 , as shown in FIG. 4 , resulting in a lower frequency serpentine path 29 .
  • FIG. 4A shows an embodiment in which several walls have been removed in major part, resulting in the passage 28 following a wide parallel path 29 across the cells 24 , corresponding to FIG. 2A .
  • the passage 28 or path 29 may also be serpentine in the plane perpendicular to the cells, as shown in the plan view of FIG. 5 .
  • the plurality of closed cells 24 in the plan view of FIG. 5 is arranged in a generally serpentine path 29 in the plane perpendicular to the common direction of the cells 23 .
  • the fluid passage 28 may thus be serpentine at a relatively higher frequency in the direction in and out of the plane of FIG. 5 , and at a relatively lower frequency within the plane of the figure, or in cases like that of FIGS. 2A and 4A , at the relatively lower frequency only.
  • Additional cells of cells 24 in a grouping 25 of more than one cell in width, if desired, may be plugged around the entry and exit ports 30 of the passage 28 , as shown in FIGS. 1 and 5 . These additional plugged cells can provide support for an O-ring seal or a fired-frit seal or other sealing system for providing a fluidic connection to the passage 28 .
  • side walls 58 may be provided on the body 20 , with ports 30 therein through which to access the passage 28 .
  • the extruded body or honeycomb 20 may be any appropriate material but is most desirably formed of an extruded glass, glass-ceramic, or ceramic material for durability and chemical inertness.
  • Alumina ceramic is generally preferred as having good strength, good inertness, and higher thermal conductivity than glass and some ceramics. Greater detail concerning general materials and fabrication procedures developed by the present inventor and/or colleagues of the present inventor may be found in PCT Publication No. WO 2008/121390, assigned to the present assignee.
  • FIGS. 7 and 8 are cross-sectional views of a fluidically connected reactor or reactor component 12 showing sample connections useful for end ports and side ports on the body 20 , respectively.
  • a fluid housing 40 supports the extruded body via seals 42 .
  • the housing 40 may comprise a single unit enclosing the extruded body, or the portions 40 A may optionally be excluded.
  • a passage 48 is formed through the open cells 22 shown in FIGS. 1 and 5 , in cooperation with the housing 40 .
  • Passage 28 in the body 20 is accessed via conduits 60 through seals 43 .
  • Still other seals 42 seal openings in the housing 40 through which conduits 60 pass.
  • FIG. 8 is similar to FIG. 7 , but less seals are required, and no seal is needed directly between the two passages 28 , 48 . Seal materials may thus be optimized independently for the materials to be flowed in each path, and seal failures will not result in materials from the two passages 28 , 48 intermixing.
  • the passage 28 and/or the passage 48 may be provided with catalyst embedded in the extruded body 20 or coated within the respective passage or within the cells of the respective passage, as desired.
  • FIG. 5 shows a simple serpentine path 29 of the passage 28 that covers most of the first end 32 of the body 20 .
  • This serpentine pattern path 29 positions a long passage 28 beside a short passage in the fowl of cells 22 , and repeats this layout configuration across the entire honeycomb body 20 .
  • the particular path 29 of FIG. 5 is just one of a class of serpentine paths that may be implemented to provide a long passage 28 through the honeycomb body 20 .
  • FIGS. 9 and 10 are the first of such plan-view, semi-schematic diagrams, of path types A and B respectively. Each subsequent additional path type is likewise labeled with a letter for ease of reference.
  • FIGS. 9 and 10 showing path types A and B, respectively, a portion of a first end of a body 20 is represented, with cells 23 , separated by walls 82 , extending in a common direction within the body 20 , into the plane of the figure.
  • Arrows 80 show the path 29 of the passage 28 and depict the direction of fluid flow.
  • foreground ones of arrows 80 correspond to locations where walls at the first end of the body 20 are reduced in height to form U-bend turns
  • background ones of arrows 80 correspond to location where walls at the second end of the body are reduced in height to form U-bend turns.
  • An “x” in a cell represents fluid flow downward into the plane of the figure, while an “o” represents fluid flow upward out of the plane of the figure.
  • the entire diagram pattern A shown in FIG. 9 can be a single sub-path unit pattern that is repeated across an end of a honeycomb body 20 .
  • additional paths not shown are used near the perimeter of a honeycomb body 20 to link path or paths 29 together into one or more larger paths, or to provide access to the passages 28 , or both, in order to form one or more continuous passages 28 through the honeycomb body 20 .
  • simple up and down passages 28 are shown, like that of FIG. 3 .
  • the passage configurations of FIGS. 10 and 11 (explained below), as well as others, can also be employed with the various patterns shown herein (e.g. three parallel cells up and three parallel cells down).
  • FIG. 10 showing path type B, the entire shown portion of the path or paths 29 of the passage or passages 28 is represented, by a pair of foreground arrows 80 .
  • FIG. 11 in the direction along the path or paths 29 , two background arrows 80 in a row are followed by two foreground arrows 80 , as two cells with “o” markings are followed by two with “x” markings, indicating a serpentine passage along the common direction of the cells 23 like the passage 28 shown in FIG. 4 .
  • FIGS. 9 and 10 depict two straight configurations, Straight 1 - 1 (Pattern A) and Straight 1 - 2 (Pattern B). Still other straight path configurations have double-width reactant cell path configurations (patterns C and D of FIGS. 11 and 12 and triple-width reactant cell path configurations (patterns E and F of FIGS. 13 and 14 , respectively).
  • the pattern of alternation of straight reactant and heat exchange cell paths can modified by integrating two or more patterns into a larger pattern, as shown in FIG. 15 , where pattern G is a Straight 2 - 1 - 1 - 1 pattern.
  • Reactant channels can be arranged in non-straight configurations by introducing turns along the flow path.
  • An example is shown in FIG. 16 , where the reactant cell bend path follows a simple serpentine in parallel to a set of open, typically heat exchange cells. This serpentine path is referred to as a 1 ⁇ 1 path because the bend extends one cell in the left-right direction, performs a 90 degree turn, extends one cell in the downward direction, and then performs another 90 degree turn.
  • a nomenclature has been developed to categorize various serpentine layout patterns.
  • the format is: Serpentine X-Y-H-S where X is the number of left-right direction cells the serpentine follows before turning, Y is the number of downward direction cells the serpentine follows before turning, H is the number of heat exchange channel columns and S is the number of cells the next reactant channel serpentine to the right is shifted downward relative to current reactant channel serpentine. (If S is zero then this value may be omitted.)
  • FIGS. 16 and 17 presents two serpentine reactant channel paths (patterns H and I) denoted as Serpentine 1 - 1 - 1 and Serpentine 1 - 1 - 2 .
  • Channel patterns can be created that include U-turns in a more complex configuration than those presented above. These patterns are called irregular even though they can be arranged in a regular array to provide a reactant channel path that covers a large portion of the substrate end face. In general these patterns are intended for applications where high reactant channel utilization is required and heat exchange performance may be relaxed. This operating point may be desirable at certain points along the reaction passage path, such as in a region near the end of a reactor where most of the reaction has already progressed to completion but additional residence time is required.
  • FIGS. 28 and 29 present a path pattern (Path T) that fills a 3 ⁇ 3 cell region with eight reactant channels and one heat exchange channel, and a second path pattern (Path U) that fills a 3 ⁇ 4 cell region with eleven reactant channels and one heat exchange channel.
  • Another path pattern is shown in FIG. 30 (Path V) where a 4 ⁇ 4 cell region is filled with fourteen reactant cells and two heat exchange cells.
  • Table 1 below presents a summary of geometrical performance parameters for all reactant channel patterns presented above (Paths A-V) of FIGS. 9-30 .
  • the first two columns provide the pattern designation code and pattern reference letter for the particular pattern.
  • the next five columns provide information on the following geometrical parameters relating to the unit pattern, where the unit pattern represents the minimum range of cells that can be repeated to reproduce the unit pattern across the honeycomb body end face: (1) Pattern Width: number of cell columns in the unit pattern; (2) Pattern Height: number of cell rows in the unit pattern; (3) Total Cells: total cells in the unit pattern (rows times columns for these patterns); (4) Reactant Cells: number of reactant cells in the pattern; (5) HE cells: number of heat exchange cells in the pattern.
  • the next column provides the reactant cell utilization factor, which is the ratio of the number of reactant cells to the total number of cells in the unit pattern.
  • the last two columns provide geometrical information on the average and maximum distance between each reactant cell in the pattern and the closest heat exchange cell, in units of cell pitch. These two parameters provide a coarse estimate of the heat exchange performance, since increased distance between reactant cells and heat exchange cells will decrease heat exchange performance. This correlation was confirmed by heat exchange performance modeling for the straight pattern configurations.
  • FIG. 31 A graphical illustration of one performance tradeoff associated with Paths A-V is provided in FIG. 31 , where calculated values of mean distance from reactant cell to heat exchange cell are plotted on the vertical axis against reactant cell utilization factor on the horizontal axis.
  • the straight patterns are shown with open diamonds, the serpentine with smaller filled diamonds, and the irregular with triangles.
  • the dashed black line 100 through or near the points for some of the patterns delineates a design tradeoff curve between local heat transfer performance and reactant cell utilization.
  • a designer may select these configurations to meet target honeycomb-body reactor performance requirements.
  • the remaining patterns appear sub-optimal in this particular tradeoff, but they may still be desirable if a particular local heat transfer performance is required for a given application independent of reactant channel utilization performance.
  • FIG. 31 A graphical illustration of one performance tradeoff associated with Paths A-V is provided in FIG. 31 , where calculated values of mean distance from reactant cell to heat exchange cell are plotted on the vertical axis against reactant cell utilization factor on the horizontal axis.
  • the straight patterns are shown with open diamonds, the serpentine with smaller filled diamonds, and the irregular with triangles.
  • the dashed black line 100 through or near the points for some of the patterns delineates a design tradeoff curve between local heat transfer performance and reactant cell utilization.
  • a designer may select these configurations to meet target honeycomb-body reactor performance requirements.
  • the remaining patterns appear sub-optimal in this particular tradeoff, but they may still be desirable if a particular local heat transfer performance is required for a given application independent of reactant channel utilization performance.
  • Patterns may also be compared using as a metric the ratio of reactant channel utilization to mean heat exchange channel distance. Results are plotted in FIG. 32 for the patterns A-V. The plot of FIG. 32 highlights the merits of the simple straight reactant pattern (Path A) as well as more complex serpentine layouts (Paths P, Q, O and S). This metric provides a measure of the maximum energy that may be transferred to or from fluid flowing in a reactant passage through a device with a given reactant cell pattern. It important to note that the configurations scoring highly on this metric do not necessarily provide the highest local heat transfer performance, so they may not be suitable for highly exothermic or endothermic reactions even though they maximize energy transfer for a device.
  • the present invention provides for a reactor or reactor component comprising a honeycomb structure having cells extending along a common direction and having one or more passages each extending across at least some of the cells, where the path or paths of the one or more passages, taken within a plane perpendicular to the common direction, includes or include a number of repeating sub-path units arranged in a two-dimensional array, with each sub-path unit including one or more turns or bends in the path. Turns herein are defined as any change of direction, whereas bends are two turns in succession in the same direction, without any intervening turns. Many of the patterns disclosed herein are patterns in which each sub-path unit includes one or more “bends,” and not merely one or more “turns.”
  • the present invention discloses the use, in a honeycomb-body based reactor, of repeated unit patterns (taken in the plane perpendicular to the common direction of the cells) of cells forming part of the reactant passage or passages.
  • repeated unit patterns takesn in the plane perpendicular to the common direction of the cells.
  • a reactor having one or more passages each extending across at least some cells of a honeycomb structure can be beneficially made by providing an array of cutting tools arrayed in a pattern selected so as to able to allow the cutting tools to simultaneously align with a first plurality of cell walls at a first end of the honeycomb structure.
  • the selected cell walls are in a corresponding or matching pattern to the array, the cell wall pattern having an area less than one-half of a total area of the first end of the structure.
  • the array of tools is then aligned with and used to cut the first plurality of cell walls, reducing their height, then the array of cutting tools may be aligned with and used to cut a second plurality of cell walls to reduce their height. This step-and-repeat cutting process may be repeated as many times as needed to form the lowered or cut-away cell walls required by the desired unit pattern.
  • FIG. 33 is a plan view of a portion of an end of an extruded body 20 .
  • An array 50 of cutting tools such as rotary plunge-cutting heads 52 is arranged so as to be able to simultaneously cut or reduce in height each wall requiring reduction or removal in given pattern unit of the selected pattern.
  • the array 50 is arranged in the configuration necessary to cut the walls of the top or first end for the smallest unit pattern 54 of pattern V of FIG. 30 (the facing end in FIG. 30 ).
  • the tools 52 are used in parallel, or cutting all at once, to remove the desired portion of a first plurality of cell walls, corresponding to the walls within a first unit pattern 54 A, then the tools 52 are moved to another unit pattern area pattern area such as second unit pattern 54 B, and a second plurality of cell walls corresponding to the pattern are cut.
  • long or short reach cutting tools may be employed. This is shown in the schematic diagrams of FIGS. 34 and 35 .
  • a holder 54 for a honeycomb structure 20 is mounted to an x-y moveable stage, not shown, allowing for the desired positioning of the structure 20 under the array 50 of cutting tools.
  • the array 50 of cutting tools is mounted to a vertically mobile body 56 , allowing the cutting heads to be brought into engagement with the selected walls of the body 20 .
  • short reach cutting tools may be employed, as in the diagram of FIG. 34 . Relatively short lengths of wall are removed, for example, to form passages 28 like the one shown in FIG. 3 .
  • honeycomb structures can be standardized around a set of one or more standard honeycomb structure shapes including one or more standard areas in the plane perpendicular to the common cell direction; one or more standard lengths; and one or more standard number of reactant passages extending across the cells of the honeycomb structure. Regardless of the level of standardization on these characteristics, any of the interchangeable reactors or reactor-components can have variable unit patterns of reactant cells in the plane perpendicular to the common cell direction.
  • reactors or reactor components can be standardized on any or all of many other dimensions, even down to one standard size and shape, but still have variability in the ratio of reactant passage cells to thermal control passage cells, depending on the unit cell pattern.
  • the variation in unit cell pattern is restricted to a set of two or more standard cell patterns yielding two or more standard ratios, taken in a plane perpendicular to the common direction, of thermal control passage cells to reactant passage cells.
  • a reactor or reactor system 10 is comprised of at least three reactors or reactor components 12 .
  • Each reactor component has the same size and shape and fluidic connections, but, depending upon the pattern used or selected for use within each reactor or reactor component 12 , the thermal exchange performance and other performance parameters can vary from one reactor or reactor component 12 to the next. The overall performance of the reactor or reactor system 10 can thus be optimized.
  • the present invention also offers advantages for the engineering and design of honeycomb-body based reactors or reactor components.
  • that performance may first be specified by determining the desired properties and/or distribution of properties for the reactor or reactor component.
  • Relevant properties may include, but are not limited to, such properties as heat transfer coefficient, pressure drop, ratio of total structure volume to total reactant passage volume, total area of open cells, distribution of open cells, and ratio of open cells to reactant passage cells.
  • a sub-path unit pattern may be selected that matches the desired properties to within an allowable deviation, from among a pre-characterized set of sub-path unit patterns.
  • the sub-path unit pattern that most closely matches the desired properties may be selected from the pre-characterized set of sub-path unit patterns.

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JP6324150B2 (ja) * 2013-07-23 2018-05-16 日本碍子株式会社 熱交換部材、およびセラミックス構造体
JP6158687B2 (ja) * 2013-11-05 2017-07-05 日本碍子株式会社 熱交換部材
WO2016017697A1 (fr) * 2014-07-29 2016-02-04 京セラ株式会社 Échangeur de chaleur
JP6700231B2 (ja) * 2017-10-17 2020-05-27 イビデン株式会社 熱交換器
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EP2367620A2 (fr) 2011-09-28
CN102227255B (zh) 2014-05-07
EP2367620A4 (fr) 2014-11-05
TW201038323A (en) 2010-11-01
TWI425980B (zh) 2014-02-11
WO2010062886A3 (fr) 2010-09-16
US20100132928A1 (en) 2010-06-03
WO2010062886A2 (fr) 2010-06-03

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